Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 136, Issue 40, Pages 14052-14059Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja504270d
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Funding
- National Research Foundation (NRF) of Korea [2011-0018198]
- BioNano Health-Guard Research Center - Ministry of Science, ICT & Future Planning (MSIP) of Korea as Global Frontier Project [H- GUARD_2013M3A6B2078947]
- Public Welfare & Safety Research Program through the National Research Foundation (NRF) - Ministry of Science, ICT, and Future Planning (MSIP), Korea [2011-0020957]
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The design, synthesis and control of plasmonic nanostructures, especially with ultrasmall plasmonically coupled nanogap (similar to 1 nm or smaller), are of significant interest and importance in chemistry, nanoscience, materials science, optics and nanobiotechnology. Here, we studied and established the thiolated DNA-based synthetic principles and methods in forming and controlling Au core-nanogap-Au shell structures [Au-nanobridged nanogap particles (Au-NNPs)] with various interior nanogap and Au shell structures. We found that differences in the binding affinities and modes among four different bases to Au core, DNA sequence, DNA grafting density and chemical reagents alter Au shell growth mechanism and interior nanogap-forming process on thiolated DNA-modified Au core. Importantly, poly A or poly C sequence creates a wider interior nanogap with a smoother Au shell, while poly T sequence results in a narrower interstitial interior gap with rougher Au shell, and on the basis of the electromagnetic field calculation and experimental results, we unraveled the relationships between the width of the interior plasmonic nanogap, Au shell structure, electromagnetic field and surface-enhanced Raman scattering. These principles and findings shown in this paper offer the fundamental basis for the thiolated DNA-based chemistry in forming and controlling metal nanostructures with similar to 1 nm plasmonic gap and insight in the optical properties of the plasmonic NNPs, and these plasmonic nanogap structures are useful as strong and controllable optical signal-generating nanoprobes.
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